Mapping electron dynamics in molecular H 2 using high-order-harmonic-generation time profiles

Abstract

The mechanism of the formation of doorway quasistates (transient species) prior to the start of ionization of the two-electron molecular H 2 system subjected to an eight-cycle ultrashort intense laser pulse is investigated by solving exactly the one-dimensional (1D) electronic time-dependent Schrödinger equation, including nuclear motion semiclassically. Space of the electron density of the two-electron 1D H 2 system around the nuclei is partitioned into four physicochemically significant partitions, including homolytic (e 1Hα+- Hβ+e 2)∼(e 2Hα+-Hβ+e 1) and ionic (Hα+-Hβ-)∼(Hα - Hβ+) transient species. The underlying mechanisms responsible for the formation and evolution of the homolytic and ionic transient species are explored based on probing variation of the two-electron norms of these states and their corresponding time-dependent high-order harmonic generation spectra. © 2012 American Physical Society.